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Catalyst accessibility to chemical reductants in metal-organic frameworks.

ABSTRACT: A molecular H2-evolving catalyst, [Fe2(cbdt)(CO)6] ([FeFe], cbdt = 3-carboxybenzene-1,2-dithiolate), has been attached covalently to an amino-functionalized MIL-101(Cr) through an amide bond. Chemical reduction experiments reveal that the MOF channels can be clogged by ion pairs that are formed between the oxidized reductant and the reduced catalyst. This effect is lessened in MIL-101-NH-[FeFe] with lower [FeFe] loadings. On longer timescales, it is shown that large proportions of the [FeFe] catalysts within the MOF engage in photochemical hydrogen production and the amount of produced hydrogen is proportional to the catalyst loading.

SUBMITTER: Roy S

PROVIDER: S-EPMC5836565 | biostudies-literature | 2017 Mar

REPOSITORIES: biostudies-literature

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Catalyst accessibility to chemical reductants in metal-organic frameworks.

Roy Souvik S Pascanu Vlad V Pullen Sonja S González Miera Greco G Martín-Matute Belén B Ott Sascha S

Chemical communications (Cambridge, England) 20170306 22

A molecular H2-evolving catalyst, [Fe2(cbdt)(CO)6] ([FeFe], cbdt = 3-carboxybenzene-1,2-dithiolate), has been attached covalently to an amino-functionalized MIL-101(Cr) through an amide bond. Chemical reduction experiments reveal that the MOF channels can be clogged by ion pairs that are formed between the oxidized reductant and the reduced catalyst. This effect is lessened in MIL-101-NH-[FeFe] with lower [FeFe] loadings. On longer timescales, it is shown that la ...[more]

PMID: 28261731

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